Removal and Oxidation of Low Concentration tert-Butanol from Potable Water using Nonthermal Plasma Coupled with Metal Oxide Adsorption

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL ACS ES&T engineering Pub Date : 2024-08-20 DOI:10.1021/acsestengg.4c0016610.1021/acsestengg.4c00166
Cristina E. Stere*, Maicon Delarmelina, Mbongiseni W. Dlamini, Sarayute Chansai, Philip R. Davies, Graham J. Hutchings, C. Richard A. Catlow* and Christopher Hardacre*, 
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Abstract

Taste and odor are crucial factors in evaluating the quality of drinking water for consumers. Geosmin is an example of a pollutant commonly found in potable water responsible for earthy and musty taste, and odor even at low concentrations. We have investigated the use of a hybrid two-step adsorption-mineralization process for low-level volatile organic compounds removal from potable water using dielectric barrier discharge over common metal oxides (MO). The system proposed is a proof of principle with tert-butanol (TBA) used as a model compound for geosmin removal/degradation during wastewater treatment when combined with an appropriate metal oxide adsorbent. Initial assessments of the adsorption properties of titania by density functional theory (DFT) calculations and experimental tests indicated that the adsorption of geosmin and TBA with water present results in only weak interactions between the sorbate and the metal oxide. In contrast, the DFT results show that alumina could be a suitable adsorbent for these tertiary alcohols and were reinforced by experimental studies. We find that while there is a competitive effect between the water and TBA adsorption from gaseous/liquid feed, the VOC can be removed, and the alumina will be regenerated by the reactive oxygen species (ROS) produced by a dielectric barrier discharge (DBD). The use of alumina in conjunction with NTP leads to efficient degradation of the adsorbate and the formation of oxygenated intermediates (formates, carbonates, and carboxylate-type species), which could then be mineralized for the regeneration of the adsorbent. A reaction mechanism has been proposed based on the in-situ infrared measurements and DFT calculations, while the removal of TBA with conventional heating is indicative of a gradual desorption process as a function of temperature rather than the destruction of the adsorbate. Furthermore, steady performance was observed after several adsorption–regeneration cycles, indicating no alteration of the adsorption properties of alumina during the NTP treatment and demonstrating the potential of the approach to be applied in the treatment of high throughput of water, without the challenges faced by the biocatalysts or formation of toxic byproducts.

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利用非热等离子体和金属氧化物吸附技术去除和氧化饮用水中的低浓度叔丁醇
味道和气味是评估消费者饮用水质量的关键因素。土臭素是饮用水中常见的一种污染物,即使浓度很低,也会产生泥土味和霉味以及异味。我们研究了在普通金属氧化物(MO)上使用电介质阻挡放电的两步吸附-矿化混合工艺来去除饮用水中的低浓度挥发性有机化合物。提出的系统是一个原理验证,以叔丁醇(TBA)为模型化合物,与适当的金属氧化物吸附剂相结合,在废水处理过程中去除/降解地奥辛。通过密度泛函理论(DFT)计算和实验测试对二氧化钛的吸附特性进行的初步评估表明,地奥司明和叔丁醇与水的吸附只会导致吸附剂和金属氧化物之间产生微弱的相互作用。与此相反,DFT 结果表明,氧化铝可能是这些叔醇的合适吸附剂,实验研究也证实了这一点。我们发现,虽然气态/液态进料中的水和 TBA 吸附之间存在竞争效应,但挥发性有机化合物可以被去除,而且氧化铝会被介质阻挡放电(DBD)产生的活性氧(ROS)再生。将氧化铝与 NTP 结合使用,可有效降解吸附剂并形成含氧中间产物(甲酸盐、碳酸盐和羧酸盐类),然后将其矿化,用于吸附剂的再生。根据原位红外测量和 DFT 计算提出了一种反应机制,而传统加热法去除 TBA 的过程表明,这是一个随温度变化而逐渐解吸的过程,而不是吸附剂被破坏的过程。此外,经过几个吸附-再生周期后,观察到了稳定的性能,这表明氧化铝的吸附特性在 NTP 处理过程中没有发生改变,并证明了该方法在处理高吞吐量水方面的应用潜力,同时还避免了生物催化剂所面临的挑战或有毒副产品的形成。
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ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
CiteScore
8.50
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0.00%
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期刊介绍: ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources. The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope. Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.
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